Publications

Abstract not provided.

Nearly every manufacturing and many technologies central to Sandia's business involve physical processes controlled by interfacial wetting. Interfacial forces, e.g. conjoining/disjoining pressure, electrostatics, and capillary condensation, are ubiquitous and can surpass and even dominate bulk inertial or viscous effects on a continuum level. Moreover, the statics and dynamics of three-phase contact lines exhibit a wide range of complex behavior, such as contact angle hysteresis due to surface roughness, surface reaction, or compositional heterogeneities. These thermodynamically and kinetically driven interactions are essential to the development of new materials and processes. A detailed understanding was developed for the factors controlling wettability in multicomponent systems from computational modeling tools, and experimental diagnostics for systems, and processes dominated by interfacial effects. Wettability probed by dynamic advancing and receding contact angle measurements, ellipsometry, and direct determination of the capillary and disjoining forces. Molecular scale experiments determined the relationships between the fundamental interactions between molecular species and with the substrate. Atomistic simulations studied the equilibrium concentration profiles near the solid and vapor interfaces and tested the basic assumptions used in the continuum approaches. These simulations provide guidance in developing constitutive equations, which more accurately take into account the effects of surface induced phase separation and concentration gradients near the three-phase contact line. The development of these accurate models for dynamic multicomponent wetting allows improvement in science based engineering of manufacturing processes previously developed through costly trial and error by varying material formulation and geometry modification.

Laser scanning confocal microscopy has been applied to study segregation in multi-component wetting. By labeling the two components of a blend with contrasting fluorescent dyes, the approximate local concentration can be determined from the relative fluorescence intensities. As a proof of concept, a coarsely blended mixture was imaged and parameters were adjusted to achieve good spectral separation of the two components. The technique was then applied to a well-blended drop of the two components and one component was observed to segregate to the air interface.

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Abstract not provided.

Alumina/poly(methyl methacrylate) (PMMA) nanocomposites were synthesized using 38 and 17 nm alumina nanoparticles. At an optimum weight fraction, the resulting nanocomposites display a room-temperature brittle-to-ductile transition in uniaxial tension with an increase in the strain-to-failure that averages 40% strain and the appearance of a well-defined yield point in uniaxial tension. Concurrently, the glass transition temperature (T{sub g}) of the nanocomposites drops by more than 20 C. The brittle-to-ductile transition is found to depend on poor interfacial adhesion between polymer and nanoparticle. This allows the nucleation of voids, typically by larger particles ({approx}100 nm), which subsequently expand during loading. This void formation suppresses craze formation and promotes delocalized shear yielding. In addition, the reduction in T{sub g} shrinks the shear yield envelope, further promoting this type of yield behavior. The brittle-to-ductile phenomenon is found to require both larger particles for void growth and smaller particles that induce the lowering of yield stress.

Alumina/poly(methyl methacrylate) (PMMA) nanocomposites were synthesized by an in situ free-radical polymerization process with 38 and 17 nm diameter {gamma}-alumina nanoparticles. At extremely low filler weight fractions (<1.0 wt % of 38 nm fillers or < 0.5 wt % of 17 nm fillers) the glass-transition temperature (T{sub g}) of the nanocomposites drops by 25 C when compared to the neat polymer. Further additions of filler (up to 10 wt %) do not lead to additional T{sub g} reductions. The thermal behavior is shown to vary with particle size, but this dependence can be normalized with respect to a specific surface area. The nanocomposite T{sub g} phenomenon is hypothesized to be because of nonadhering nanoparticles that serve as templates for a porous system with many internal interfaces that break up the percolating structure of dynamically heterogeneous domains recently suggested by Long, D.; and Lequeux, F. Eur Phys J E 2001, 4, 371 to be responsible for the T{sub g} reductions in polymer ultrathin films. The results also point to a far field effect of the nanoparticle surface on the bulk matrix.